Study on Stratospheric Carbonyl Sulfide Transport and Chemistry using ‘Age of Air’

2021 ◽  
Author(s):  
Chenxi Qiu ◽  
Felix Ploeger ◽  
Jens-Uwe Grooß ◽  
Marc von Hobe
Keyword(s):  
Atmospheric Chemistry ◽  
Michelson Interferometer ◽  
Carbonyl Sulfide ◽  
Polar Vortex ◽  
Lagrangian Model ◽  
Latitude Range ◽  
Mixing Ratios ◽  
Enhanced Absorption ◽  
In Situ Data

<p>Carbonyl sulfide (OCS or COS) is the longest lived and the most abundant reduced sulfur gas in the atmosphere. As chemical loss of OCS in the troposphere is slow, it can reach the stratosphere, where it is  photochemically oxidized and converted to stratospheric sulfate aerosol, being the largest source thereof in times of volcanic quiescence. Chemistry transport models show that OCS conversion occurs mainly in the ‘tropical pipe’ region, while along the lower branch of Brewer-Dobson circulation (BDC), OCS is passively transported without significant chemical loss. The OCS depleted air is transported along the upper branch of BDC and descends again at high latitudes. Using the distinct characteristics of  ‘age of air’ in the upper and lower branches of the BDC, this picture of OCS transport and especially the role of the ‘tropical pipe’ as the main region of OCS conversion can be supported by looking at the relationship between age spectra and OCS mixing ratios.</p><p>In this study, we will investigate the relation of OCS mixing ratios and mean age of air as well as mass fractions of air with different transit times using satellite-based measurements from MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) and ACE-FTS (Atmospheric Chemistry Experiment - infrared Fourier Transform Spectrometer), and age spectra of air from CLaMS (Chemical Lagrangian Model of the Stratosphere).</p><p>In addition to satellite data analysis, we will investigate the distribution of OCS in the UTLS (upper troposphere and lower stratosphere) region and its relation to the age spectra using high-resolution in-situ observations of OCS. This unique dataset was obtained during the SOUTHTRAC mission in autumn 2019 by AMICA (Airborne Mid-Infrared Cavity enhanced Absorption spectrometer) on board the HALO (High Altitude Long Range) research aircraft. Flights from the main  campaign base in Río Grande, Argentina (53.8S, 67.7W) covered a wide latitude range from 48° N to 70° S, even reaching the southern polar vortex where aged air masses having descended from high altitudes are typically found.</p><p>Our analysis of both satellite and in-situ data generally supports the established picture of OCS conversion in the ‘tropical pipe’.</p>

scholarly journals New approach to evaluate satellite derived XCO<sub>2</sub> over oceans by integrating ship and aircraft observations

2020 ◽  
Author(s):  
Astrid Müller ◽  
Hiroshi Tanimoto ◽  
Takafumi Sugita ◽  
Toshinobu Machida ◽  
Shin-ichiro Nakaoka ◽  
...  
Keyword(s):  
Carbon Cycle ◽  
Atmospheric Chemistry ◽  
Transport Model ◽  
Satellite Observations ◽  
Reference Dataset ◽  
Model Calculations ◽  
New Approach ◽  
Mixing Ratios ◽  
In Situ Data

Abstract. Satellite observations provide spatially-resolved global estimates of column-averaged mixing ratios of CO2 (XCO2) over the Earth's surface. The accuracy of these datasets can be validated against reliable standards in some areas, but other areas remain inaccessible. To date, limited reference data over oceans hinders successful uncertainty quantification or bias correction efforts, and precludes reliable conclusions about changes in the carbon cycle in some regions. Here, we propose a new approach to analyze and evaluate seasonal, interannual and latitudinal variations of XCO2 over oceans by integrating cargo-ship (SOOP, Ship Of Opportunity) and commercial aircraft (CONTRAIL, Comprehensive Observation Network for Trace gases by Airliner) observations with the aid of state-of-the art atmospheric chemistry-transport model calculations. The consistency of the in situ based column-averaged CO2 dataset (in situ XCO2) with satellite estimates was analyzed over the Western Pacific between 2014 and 2017, and its utility as reference dataset evaluated. Our results demonstrate that the new dataset accurately captures seasonal and interannual variations of CO2. Retrievals of XCO2 over the ocean from GOSAT (Greenhouse gases observing satellite: NIES v02.75, National Institute for Environmental Studies; ACOS v7.3, Atmospheric CO2 Observation from Space) and OCO-2 (Orbiting Carbon Observatory, v9r) observations show a negative bias of about 1 parts per million (ppm) in northern midlatitudes, which was attributed to measurement uncertainties of the satellite observations. The NIES retrieval had higher consistency with in situ XCO2 at midlatitudes as compared to the other retrievals. At low latitudes, it shows many fewer valid data and high scatter, such that ACOS and OCO-2 appear to provide a better representation of the carbon cycle. At different times, the seasonal cycles of all three retrievals show positive phase shifts of one month relative to the in situ data. The study indicates that even if the retrievals complement each other, remaining uncertainties limit the accurate interpretation of spatiotemporal changes in CO2 fluxes. A continuous long-term XCO2 dataset with wide latitudinal coverage based on the new approach has a great potential as a robust reference dataset for XCO2 and can help to better understand changes in the carbon cycle in response to climate change using satellite observations.

scholarly journals Exploring the atmospheric chemistry of nitrous acid (HONO) at a rural site in Southern China

2012 ◽  
Vol 12 (3) ◽  
pp. 1497-1513 ◽  
Author(s):  
X. Li ◽  
T. Brauers ◽  
R. Häseler ◽  
B. Bohn ◽  
H. Fuchs ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Nitrous Acid ◽  
Southern China ◽  
Rural Site ◽  
Pearl River Delta Region ◽  
Additional Source ◽  
Mixing Ratios ◽  
Photolysis Frequency ◽  
The Pearl River

Abstract. We performed measurements of nitrous acid (HONO) during the PRIDE-PRD2006 campaign in the Pearl River Delta region 60 km north of Guangzhou, China, for 4 weeks in June 2006. HONO was measured by a LOPAP in-situ instrument which was setup in one of the campaign supersites along with a variety of instruments measuring hydroxyl radicals, trace gases, aerosols, and meteorological parameters. Maximum diurnal HONO mixing ratios of 1–5 ppb were observed during the nights. We found that the nighttime build-up of HONO can be attributed to the heterogeneous NO2 to HONO conversion on ground surfaces and the OH + NO reaction. In addition to elevated nighttime mixing ratios, measured noontime values of ≈200 ppt indicate the existence of a daytime source higher than the OH + NO→HONO reaction. Using the simultaneously recorded OH, NO, and HONO photolysis frequency, a daytime additional source strength of HONO (PM) was calculated to be 0.77 ppb h−1 on average. This value compares well to previous measurements in other environments. Our analysis of PM provides evidence that the photolysis of HNO3 adsorbed on ground surfaces contributes to the HONO formation.

scholarly journals Validation of MIPAS IMK/IAA methane profiles

2015 ◽  
Vol 8 (12) ◽  
pp. 5251-5261 ◽  
Author(s):  
A. Laeng ◽  
J. Plieninger ◽  
T. von Clarmann ◽  
U. Grabowski ◽  
G. Stiller ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Michelson Interferometer ◽  
European Space Agency ◽  
Trace Gas ◽  
Mixing Ratios ◽  
Air Sampler ◽  
Solar Occultation ◽  
Space Agency ◽  
Scanning Imaging ◽  
Satellite Instruments

Abstract. The Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) is an infrared (IR) limb emission spectrometer on the Envisat platform. It measures trace gas distributions during day and night, pole-to-pole, over an altitude range from 6 to 70 km in nominal mode and up to 170 km in special modes, depending on the measurement mode, producing more than 1000 profiles day−1. We present the results of a validation study of methane, version V5R_CH4_222, retrieved with the IMK/IAA (Institut für Meteorologie und Klimaforschung, Karlsruhe/Instituto de Astrofisica de Andalucia, Grenada) MIPAS scientific level 2 processor. The level 1 spectra are provided by the ESA (European Space Agency) and version 5 was used. The time period covered is 2005–2012, which corresponds to the period when MIPAS measured trace gas distributions at a reduced spectral resolution of 0.0625 cm−1. The comparison with satellite instruments includes the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS), the HALogen Occultation Experiment (HALOE), the Solar Occultation For Ice Experiment (SOFIE) and the SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY). Furthermore, comparisons with MkIV balloon-borne solar occultation measurements and with air sampling measurements performed by the University of Frankfurt are presented. The validation activities include bias determination, assessment of stability, precision validation, analysis of histograms and comparison of corresponding climatologies. Above 50 km altitude, MIPAS methane mixing ratios agree within 3 % with ACE-FTS and SOFIE. Between 30 and 40 km an agreement within 3 % with SCIAMACHY has been found. In the middle stratosphere, there is no clear indication of a MIPAS bias since comparisons with various instruments contradict each other. In the lower stratosphere (below 25 km) MIPAS CH4 is biased high with respect to satellite instruments, and the most likely estimate of this bias is 14 %. However, in the comparison with CH4 data obtained from cryogenic whole-air sampler (cryosampler) measurements, there is no evidence of a high bias in MIPAS between 20 and 25 km altitude. Precision validation is performed on collocated MIPAS–MIPAS pairs and suggests a slight underestimation of its uncertainties by a factor of 1.2. No significant evidence of an instrumental drift has been found.

scholarly journals Chlorine nitrate in the atmosphere

2018 ◽  
Vol 18 (20) ◽  
pp. 15363-15386 ◽  
Author(s):  
Thomas von Clarmann ◽  
Sören Johansson
Keyword(s):  
Atmospheric Chemistry ◽  
Infrared Emission ◽  
Chlorine Nitrate ◽  
Rotational Bands ◽  
In Situ Techniques ◽  
Mixing Ratios ◽  
Gas Phase Chemistry ◽  
Polar Stratosphere ◽  
Phase Chemistry

Abstract. This review article compiles the characteristics of the gas chlorine nitrate and discusses its role in atmospheric chemistry. Chlorine nitrate is a reservoir of both stratospheric chlorine and nitrogen. It is formed by a termolecular reaction of ClO and NO2. Sink processes include gas-phase chemistry, photo-dissociation, and heterogeneous chemistry on aerosols. The latter sink is particularly important in the context of polar spring stratospheric chlorine activation. ClONO2 has vibrational–rotational bands in the infrared, notably at 779, 809, 1293, and 1735 cm−1, which are used for remote sensing of ClONO2 in the atmosphere. Mid-infrared emission and absorption spectroscopy have long been the only concepts for atmospheric ClONO2 measurements. More recently, fluorescence and mass spectroscopic in situ techniques have been developed. Global ClONO2 distributions have a maximum at polar winter latitudes at about 20–30 km altitude, where mixing ratios can exceed 2 ppbv. The annual cycle is most pronounced in the polar stratosphere, where ClONO2 concentrations are an indicator of chlorine activation and de-activation.

scholarly journals Characterization of Aura TES carbonyl sulfide retrievals over ocean

2014 ◽  
Vol 7 (1) ◽  
pp. 163-172 ◽  
Author(s):  
L. Kuai ◽  
J. Worden ◽  
S. S. Kulawik ◽  
S. A. Montzka ◽  
J. Liu
Keyword(s):  
Carbonyl Sulfide ◽  
Systematic Errors ◽  
Retrieval Algorithm ◽  
Aircraft Measurements ◽  
Random Errors ◽  
Mauna Loa ◽  
In Situ Data ◽  
Peak Sensitivity

Abstract. We present a description of the NASA Aura Tropospheric Emission Spectrometer (TES) carbonyl sulfide (OCS) retrieval algorithm for oceanic observations, along with evaluation of the biases and uncertainties using aircraft profiles from the HIPPO (HIAPER Pole-to-Pole Observations) campaign and data from the NOAA Mauna Loa site. In general, the OCS retrievals (1) have less than 1.0 degree of freedom for signals (DOFs), (2) are sensitive in the mid-troposphere with a peak sensitivity typically between 300 and 500 hPa, (3) but have much smaller systematic errors from temperature, CO2 and H2O calibrations relative to random errors from measurement noise. We estimate the monthly means from TES measurements averaged over multiple years so that random errors are reduced and useful information about OCS seasonal and latitudinal variability can be derived. With this averaging, TES OCS data are found to be consistent (within the calculated uncertainties) with NOAA ground observations and HIPPO aircraft measurements. TES OCS data also captures the seasonal and latitudinal variations observed by these in situ data.

scholarly journals Middle atmospheric water vapour and dynamics in the vicinity of the polar vortex during the Hygrosonde-2 campaign

2009 ◽  
Vol 9 (13) ◽  
pp. 4407-4417 ◽  
Author(s):  
S. Lossow ◽  
M. Khaplanov ◽  
J. Gumbel ◽  
J. Stegman ◽  
G. Witt ◽  
...  
Keyword(s):  
Water Vapour ◽  
Middle Atmosphere ◽  
Polar Vortex ◽  
The Arctic ◽  
Small Scale ◽  
Air Masses ◽  
Mixing Ratios ◽  
Water Vapour Concentration ◽  
Wind Shears

Abstract. The Hygrosonde-2 campaign took place on 16 December 2001 at Esrange/Sweden (68° N, 21° E) with the aim to investigate the small scale distribution of water vapour in the middle atmosphere in the vicinity of the Arctic polar vortex. In situ balloon and rocket-borne measurements of water vapour were performed by means of OH fluorescence hygrometry. The combined measurements yielded a high resolution water vapour profile up to an altitude of 75 km. Using the characteristic of water vapour being a dynamical tracer it was possible to directly relate the water vapour data to the location of the polar vortex edge, which separates air masses of different character inside and outside the polar vortex. The measurements probed extra-vortex air in the altitude range between 45 km and 60 km and vortex air elsewhere. Transitions between vortex and extra-vortex usually coincided with wind shears caused by gravity waves which advect air masses with different water vapour volume mixing ratios. From the combination of the results from the Hygrosonde-2 campaign and the first flight of the optical hygrometer in 1994 (Hygrosonde-1) a clear picture of the characteristic water vapour distribution inside and outside the polar vortex can be drawn. Systematic differences in the water vapour concentration between the inside and outside of the polar vortex can be observed all the way up into the mesosphere. It is also evident that in situ measurements with high spatial resolution are needed to fully account for the small-scale exchange processes in the polar winter middle atmosphere.

scholarly journals Characterization of aura tropospheric emissions spectrometer carbonyl sulfide retrievals

2013 ◽  
Vol 6 (4) ◽  
pp. 6975-7003
Author(s):  
L. Kuai ◽  
J. Worden ◽  
S. S. Kulawik ◽  
S. A. Montzka ◽  
J. Liu
Keyword(s):  
Carbonyl Sulfide ◽  
Systematic Errors ◽  
Retrieval Algorithm ◽  
Aircraft Measurements ◽  
Random Errors ◽  
Mauna Loa ◽  
In Situ Data ◽  
Peak Sensitivity

Abstract. We present a description of the Tropospheric Emission Spectrometer (TES) carbonyl sulfide (OCS) retrieval algorithm, along with evaluation of the biases and uncertainties against aircraft profiles from the HIPPO campaign and data from the NOAA Mauna Loa site. In general, the OCS retrievals (1) have less than 1.0 degree of freedom for signals (DOFs), (2) are sensitive in the mid-troposphere with a peak sensitivity typically between 300 to 500 hPa, (3) but have much smaller systematic errors from temperature, CO2 and H2O calibrations relative to random errors from measurement noise. Here we estimate the monthly means from TES measurements averaged over multiple years so that random errors are reduced and useful information about OCS seasonal and latitudinal variability can be derived. With this averaging, TES OCS data are found to be consistent (within the calculated uncertainties) with NOAA ground observations and HIPPO aircraft measurements. TES OCS data also captures the seasonal and latitudinal variations observed by these in situ data.

scholarly journals Observations of filamentary structures near the vortex edge in the Arctic winter lower stratosphere

2013 ◽  
Vol 13 (21) ◽  
pp. 10859-10871 ◽  
Author(s):  
C. Kalicinsky ◽  
J.-U. Grooß ◽  
G. Günther ◽  
J. Ungermann ◽  
J. Blank ◽  
...  
Keyword(s):  
Cross Sections ◽  
Transport Model ◽  
Stratospheric Ozone ◽  
Polar Vortex ◽  
Lagrangian Model ◽  
The Arctic ◽  
Small Scale ◽  
Air Mass ◽  
Mixing Ratios ◽  
Passive Tracers

Abstract. The CRISTA-NF (Cryogenic Infrared Spectrometers and Telescope for the Atmosphere – New Frontiers) instrument is an airborne infrared limb sounder operated aboard the Russian research aircraft M55-Geophysica. The instrument successfully participated in a large Arctic aircraft campaign within the RECONCILE (Reconciliation of essential process parameters for an enhanced predictability of Arctic stratospheric ozone loss and its climate interactions) project in Kiruna (Sweden) from January to March 2010. This paper concentrates on the measurements taken during one flight of the campaign, which took place on 2 March in the vicinity of the polar vortex. We present two-dimensional cross-sections of derived volume mixing ratios for the trace gases CFC-11, O3, and ClONO2 with an unprecedented vertical resolution of about 500 to 600 m for a large part of the observed altitude range (≈ 6–19 km) and a dense horizontal sampling along flight direction of ≈ 15 km. The trace gas distributions show several structures, for example a part of the polar vortex and a vortex filament, which can be identified by means of O3–CFC-11 tracer–tracer correlations. The observations made during this flight are interpreted using the chemistry and transport model CLaMS (Chemical Lagrangian Model of the Stratosphere). Comparisons of the observations with the model results are used to assess the performance of the model with respect to advection, mixing, and the chemistry in the polar vortex. These comparisons confirm the capability of CLaMS to reproduce even very small-scale structures in the atmosphere, which partly have a vertical extent of only 1 km. Based on the good agreement between simulation and observation, we use artificial (passive) tracers, which represent different air mass origins (e.g. vortex, tropics), to further analyse the CRISTA-NF observations in terms of the composition of air mass origins. These passive tracers clearly illustrate the observation of filamentary structures that include tropical air masses. A characteristic of the Arctic winter 2009/10 was a sudden stratospheric warming in December that led to a split of the polar vortex. The vortex re-established at the end of December. Our passive tracer simulations suggest that large parts of the re-established vortex consisted to about 45% of high- and mid-latitude air.

scholarly journals MIPAS-STR measurements in the Arctic UTLS in winter/spring 2010: instrument characterization, retrieval and validation

2012 ◽  
Vol 5 (6) ◽  
pp. 1205-1228 ◽  
Author(s):  
W. Woiwode ◽  
H. Oelhaf ◽  
T. Gulde ◽  
C. Piesch ◽  
G. Maucher ◽  
...  
Keyword(s):  
Cross Sections ◽  
Stratospheric Ozone ◽  
Trace Gases ◽  
Michelson Interferometer ◽  
Polar Vortex ◽  
The Arctic ◽  
Radiometric Calibration ◽  
Mid Infrared ◽  
Mean Differences

Abstract. The mid-infrared FTIR-limb-sounder Michelson Interferometer for Passive Atmospheric Sounding–STRatospheric aircraft (MIPAS-STR) was deployed onboard the research aircraft M55 Geophysica during the RECONCILE campaign (Reconciliation of Essential Process Parameters for an Enhanced Predictability of Arctic Stratospheric Ozone Loss and its Climate Interactions) in the Arctic winter/spring 2010. From the MIPAS-STR measurements, vertical profiles and 2-dimensional vertical cross-sections of temperature and trace gases are retrieved. Detailed mesoscale structures of polar vortex air, extra vortex air and vortex filaments are identified in the results at typical vertical resolutions of 1 to 2 km and typical horizontal sampling densities of 45 or 25 km, depending on the sampling programme. Results are shown for the RECONCILE flight 11 on 2 March 2010 and are validated with collocated in-situ measurements of temperature, O3, CFC-11, CFC-12 and H2O. Exceptional agreement is found for the in-situ comparisons of temperature and O3, with mean differences (vertical profile/along flight track) of 0.2/−0.2 K for temperature and −0.01/0.05 ppmv for O3 and corresponding sample standard deviations of the mean differences of 0.7/0.6 K and 0.1/0.3 ppmv. The comparison of the retrieved vertical cross-sections of HNO3 from MIPAS-STR and the infrared limb-sounder Cryogenic Infrared Spectrometers and Telescopes for the Atmosphere–New Frontiers (CRISTA–NF) indicates a high degree of agreement. We discuss MIPAS-STR in its current configuration, the spectral and radiometric calibration of the measurements and the retrieval of atmospheric parameters from the spectra. The MIPAS-STR measurements are significantly affected by continuum-like contributions, which are attributed to background aerosol and broad spectral signatures from interfering trace gases, and are important for mid-infrared limb-sounding in the Upper Troposphere/Lower Stratosphere (UTLS) region. Taking into consideration continuum-like effects, we present a scheme suitable for accurate retrievals of temperature and an extended set of trace gases, including the correction of a systematic line-of-sight offset.

scholarly journals A framework for comparing remotely sensed and in-situ CO<sub>2</sub> concentrations

2008 ◽  
Vol 8 (1) ◽  
pp. 1549-1588 ◽  
Author(s):  
R. Macatangay ◽  
T. Warneke ◽  
C. Gerbig ◽  
S. Körner ◽  
R. Ahmadov ◽  
...  
Keyword(s):  
Carbon Dioxide ◽  
Transport Model ◽  
Remotely Sensed ◽  
Infrared Spectrometry ◽  
Remotely Sensed Data ◽  
Solar Absorption ◽  
Mixing Ratios ◽  
In Situ Data ◽  
Global Calibration

Abstract. A framework that allows validating CO2 column averaged volume mixing ratios (VMRs) retrieved from ground-based solar absorption measurements using Fourier transform infrared spectrometry (FTS) against measurements made in-situ (such as from aircrafts and tall towers) has been developed. Since in-situ measurements are done frequently and at high accuracy on the global calibration scale, linking this scale with FTS total column retrievals ultimately provides a calibration scale for remote sensing. FTS, tower and aircraft data were analyzed from measurements during the CarboEurope Regional Experiment Strategy (CERES) from May to June 2005 in Biscarrosse, France. Carbon dioxide VMRs from the MetAir Dimona aircraft, the TM3 global transport model and Observations of the Middle Stratosphere (OMS) balloon based experiments were combined and integrated to compare with FTS measurements. The comparison agrees fairly well with differences resulting from the spatial variability of CO2 around the FTS as measured by the aircraft. Additionally, the Stochastic Time Inverted Lagrangian Transport (STILT) model served as a "transfer standard" between the in-situ data measured at a co-located tower and the remotely sensed data from the FTS. The variability of carbon dioxide VMRs was modeled well by STILT with differences coming partly from uncertainties in the spatial variation of carbon dioxide.

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